Dynamic Activation of Adsorbed Intermediates via Axial Traction for the Promoted Electrochemical CO<sub>2</sub> Reduction
Xinyue Wang, Yu Wang, Xiahan Sang, Wanzhen Zheng, Shihan Zhang, Ling Shuai, Bin Yang, Zhongjian Li, Jianmeng Chen, Lecheng Lei, Nadia Mohd Adli, Michael K.H. Leung, Ming Qiu, Gang Wu, Yang Hou
Abstract
Abstract Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M‐N 4 ) to accelerate overall reaction dynamics of the electrochemical CO 2 reduction reaction (CO 2 RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M‐N 4 moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni‐N 4 ‐O/C). The Ni‐N 4 ‐O/C electrocatalyst exhibited excellent CO 2 RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at −0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from −0.5 to −1.1 V. The superior CO 2 RR activity is due to the Ni‐N 4 ‐O active moiety composed of a Ni‐N 4 site with an additional oxygen atom that induces an axial traction effect.